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Charge transfer to solvent dynamics at the ambient water/air interface.

Nowakowski, P. J. and Woods, D. A. and Verlet, J. R. R. (2016) 'Charge transfer to solvent dynamics at the ambient water/air interface.', Journal of physical chemistry letters., 7 (20). pp. 4079-4085.


Electron-transfer reactions at ambient aqueous interfaces represent one of the most fundamental and ubiquitous chemical reactions. Here the dynamics of the charge transfer to solvent (CTTS) reaction from iodide was probed at the ambient water/air interface by phase-sensitive transient second-harmonic generation. Using the three allowed polarization combinations, distinctive dynamics assigned to the CTTS state evolution and to the subsequent solvating electron-iodine contact pair have been resolved. The CTTS state is asymmetrically solvated in the plane of the surface, while the subsequent electron solvation dynamics are very similar to those observed in the bulk, although slightly faster. Between 3 and 30 ps, a small phase shift distinguishes an electron bound in a contact pair with iodine and a free hydrated electron at the water/air interface. Our results suggest that the hydrated electron is fully solvated in a region of reduced water density at the interface.

Item Type:Article
Full text:(AM) Accepted Manuscript
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Publisher statement:This document is the Accepted Manuscript version of a Published Work that appeared in final form in Journal of physical chemistry letters, copyright © American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see
Date accepted:29 September 2016
Date deposited:31 October 2016
Date of first online publication:03 October 2016
Date first made open access:03 October 2017

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